Study of Wavepacket Dynamics in Rubidium Vapor by Means of Time-Frequency Analysis

Wavepackets are excited in rubidium vapor by intense ultrashort (∼100 fs) pulses centered at a wavelength of 620 nm or 770 nm. The generated atomic wavepackets are optically detected via a pump-probe experiment based on axially phase-matched parametric four-wave mixing (FWM). This nonlinear process results in coherent ultraviolet (UV) or violet emission that carries information about the relative number densities of the excited states. The frequency spectrum of the UV/violet signal intensity, recorded while varying the pump-probe time delay, shows the presence of quantum beats between energy levels involved in the FWM process. The time-frequency analysis of that temporal UV/violet data is done by means of the short-time Fourier transform that leads to retrieval of the temporal evolution of amplitude and phase of the quantum beats. The observed dynamics suggest that not only atomic but also molecular ( Rb*2 ) wavepackets are generated, and that the temporal history of the amplitude of the quantum beats reflects the production of the excited atomic fragments of Rb*2 dissociation. More precisely, changes in the Rb excited state number densities alter the third-order nonlinear susceptibility chi(3) of the Rb vapor, which affects generation of the output signal wave by FWM. Dissociation into several product states is detected, and their branching ratios are estimated. Thus, atomic wavepackets, combined with FWM, appear to be a sensitive new multichannel spectroscopic means to study the fundamental process of molecular dissociation.

Name thesis:degree_name

Ph.D.

Level thesis:degree_level

Dissertation

Discipline thesis:degree_discipline

Electrical Engineering

Grantor

University of Illinois at Urbana-Champaign

Year dc:date

2015

Author dc:creator

• Senin, Andrey Aleksandrovich

Contributors dc:contributor

• James Gary Eden

• Physics, Molecular

Language dc:language

eng

Identifier

(MiAaPQ)AAI3101967

OAI identifier oai:identifier

oai:www.ideals.illinois.edu:2142/80841